We are developing relaxometry and related methods to probe macromolecular compartments withing cartilage, brain, and muscle. The goal is to identify mobility, concentration, and exchange between hydration compartments within tissue. It is well-known that changes in these features play a prominent role in pathology associated with both aging and disease. We are using compressed sensing as a modality to move to a more translational aspect to these studies. Overall, this work should expand the capability of chemical-physical probes of disease, permitting evaluation of progression and of therapies using noninvasive magnetic resonance technology.